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Organic electro-optic (E-O) materials have attracted considerable research attention in the past 20 years due to their rising potentials in a lot of novel photonic applications, such as high-speed telecommunication, terahertz generation and ultra-fast optical interconnections. In order to gain the Pockels effect based E-O activity, the centro-symmetry of amorphous organic E-O materials needs to be removed by a poling process, which introduces orientation to the polar chromophores by applying high electric field. After poling, this collective orientation is subject to a slow decay over time, which can eventually dissipate the E-O activity of the poled material. Thus the study of how to effectively introduce and preserve chromophore orientation forms an important part of the research of organic E-O materials. This dissertation starts with a general introduction to the field in Chapter 1, which includes the basic nonlinear optics, the design rules for material development, and the potential applications as well as the motivation and scope of this dissertation. Chapter 2 of this dissertation focuses on a barrier layer approach to improve the poling efficiency of E-O polymers. First of all, high conduction current from excessive charge injection is identified as a fundamental challenge of effective poling. After analyzing the conduction mechanism, we introduce a sol-gel derived thin titanium dioxide (TiO<sub>2</sub>) layer that can significantly block excessive charge injection and reduce the leakage current during high field poling. Ultralarge E-O coefficients, up to 160-350 pm/V at 1310 nm have been achieved by poling with such a barrier, which are 26%-40% higher than the results poled without such a TiO<sub>2</sub> layer. This enhancement is explained by the suppressed charge injection and space charge accumulation by the insertion of the high injection barrier from the TiO<sub>2</sub> barrier layer. In Chapter 3, the impact of the inserted barrier layer on the temporal alignment stability of E-O polymers is discussed. Considerable stability enhancement is confirmed using both standard 500-hour temporal alignment stability test at 85 °C and thermally stimulated discharge method. We suggest that the enhancement comes from improved stability of the screening charge. During poling the additional barrier layer helps to lower the injection and thus the space charge accumulation. And this reduced space charge accumulation further helps to replace the space charge part in the total formulation of screening charge with more stable interface trapped charge. We thus expand this knowledge to a group of other materials that can also block excessive charge injection and suppressed space charge accumulation, including dielectric polymers polyvinyl alcohol (PVA), poly(4-vinylphenol) (PVP) and TOPAS as well as ferroelectric polymer poly(vinylidene fluoride-co-trifluoroethylene) (P(VDF-TrFE), 65/35 copolymer), which differ largely from the others in dielectric constant, conductivity and surface properties. The only common feature of them is that they all lowered the charge injection and leakage current for 1-2 orders during poling. On every buffer layer we tried, similar trend of stability enhancement is found. These results suggest that the observed temporal stability enhancement is indeed an effect from the abovementioned mechanism. Chapter 4 focuses on the development of an innovative new poling method, which utilizes pyroelectric effect instead of external power sources to overcome the limitations of conventional contact poling and corona poling. With careful theory assisted design, we developed a reliable protocol to efficiently introduce dipole orientation in organic E-O materials by heating and cooling them with detachable pyroelectric crystals. This new method can potentially improve the process adaptability of organic E-O materials in a variety of photonic devices. Large Pockels coefficients (up to 81 pm/V at 1.3 micron) have been successfully achieved in thin films poled using this method. The effective fields in these experiments are estimated to be around 0.5 to 0.9 MV/cm, which agree well with the electrostatics analysis using an idealized model. The same method is directly applied to surface modified hybrid polymer silicon slot waveguide ring-resonator modulators devices. A 25 pm/V tunability of resonance peak wavelength shift has been realized, which was higher than any reported results in similar devices. Chapter 5 discusses about the possible application of the pyroelectric poling in a multi-stack waveguide device architecture. A long-existing challenge to pole E-O polymer based photonic devices is how to effectively drop the poling voltage to the core layer, which is usually sandwiched between two dielectric claddings. In the past, this was done by using relatively conductive claddings, which on the other hand can bring larger optical loss and dielectric loss to the waveguide. Thus careful engineering compromise must be made between better poling efficiency and lower loss. Pyroelectric poling as discussed in Chapter 4 opens up new possibilities. In this chapter, it is demonstrated that E-O polymer films can be poled even with 3 orders thicker dielectric layer in circuit using pyroelectric poling. The theoretical analysis matches well with the experimental results. It could provide new insight to the research of poling E-O polymers in hybrid photonic devices, where the E-O materials form intimate contact with different types of materials in the system.